title: β-AgAl(1-x)Ga(x)O2 solid-solution photocatalysts: continuous modulation of electronic structure toward high-performance visible-light photoactivity.
abstract: A series of β-AgAl(1-x)Ga(x)O(2) solid-solution materials were explored as novel visible-light-sensitive photocatalysts. These Ag-based solid solutions crystallize in a homogeneous crystal structure with orthorhombic symmetry but possess continuously modulated band gaps from 2.19 to 2.83 eV by decreasing the ratios of Ga/Al. Their photoactivities for iso-propanol degradation were found to be dependent on the variation of chemical compositions. Among them, the β-AgAl(0.6)Ga(0.4)O(2) sample showed the highest photocatalytic performance, which simultaneously exhibited 35 and 63 times higher activities than two terminus materials, β-AgAlO(2) and β-AgGaO(2), respectively. The apparent quantum efficiency of this sample for iso-propanol photodegradation achieved up to 37.3% at the wavelength of 425 ± 12 nm. The theoretical calculation based on density functional theory demonstrated that the levels of valence band maximum of β-AgAl(1-x)Ga(x)O(2) are similar, but the levels of conduction band minimum are gradually negatively shifted with the increase of the ratio of Ga/Al, thereby continuously narrowing the band gap. Nevertheless, the highest activity observed on β-AgAl(0.6)Ga(0.4)O(2) may be attributed to its optimized band structure, which adapts the balance between effective visible-light absorption and adequate redox potentials.
authors.affiliation: Photocatalytic Materials Center (PCMC), National Institute for Materials Science (NIMS), 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047, Japan.
authors.forename: Shuxin
authors.initials: S
authors.lastname: Ouyang
authors.forename: Jinhua
authors.initials: J
authors.lastname: Ye